This paper is devoted to the iron corrosion phenomena induced by the α (4He2+) water radiolysis species studied in conjunction with the production/consumption of H2 at the solid/solution interface. On one hand, the solid surface is characterized during the 4He2+ ions irradiation by in situ Raman spectroscopy; on another hand, the H2 gas produced by the water radiolysis is monitored by ex situ gas measurements. The 4He2+ ions irradiation experiments are provided either by the CEMHTI (E = 5.0 MeV) either by the ARRONAX (E = 64.7 MeV) cyclotron facilities. The iron corrosion occurs only under irradiation and can be slowed down by H2 reductive atmosphere. Pure iron and carbon steel solids are studied in order to show two distinct behaviors of t...